Title: Electrical control of 2D magnetism in bilayer CrI 3

Controlling magnetism via electric fields addresses fundamental questions of magnetic phenomena and phase transitions, and enables the development of electrically coupled spintronic devices, such as voltage-controlled magnetic memories with low operation energy. Previous studies on dilute magnetic semiconductors such as (Ga,Mn)As and (In,Mn)Sb have demonstrated large modulations of the Curie temperatures and coercive fields by altering the magnetic anisotropy and exchange interaction. Owing to their unique magnetic properties, the recently reported two-dimensional magnets provide a new system for studying these features. For instance, a bilayer of chromium triiodide (CrI 3) behaves as a layered antiferromagnet with a magnetic field-driven metamagnetic transition. Here, we demonstrate electrostatic gate control of magnetism in CrI 3 bilayers, probed by magneto-optical Kerr effect (MOKE) microscopy. At fixed magnetic fields near the metamagnetic transition, we realize voltage-controlled switching between antiferromagnetic and ferromagnetic states. At zero magnetic field, we demonstrate a time-reversal pair of layered antiferromagnetic states that exhibit spin-layer locking, leading to a linear dependence of their MOKE signals on gate voltage with opposite slopes. Here, our results allow for the exploration of new magnetoelectric phenomena and van der Waals spintronics based on 2D materials.

@article{osti_1436027,
title = {Electrical control of 2D magnetism in bilayer CrI3},
author = {Huang, Bevin and Clark, Genevieve and Klein, Dahlia R. and MacNeill, David and Navarro-Moratalla, Efren and Seyler, Kyle L. and Wilson, Nathan and McGuire, Michael A. and Cobden, David H. and Xiao, Di and Yao, Wang and Jarillo-Herrero, Pablo and Xu, Xiaodong},
abstractNote = {Controlling magnetism via electric fields addresses fundamental questions of magnetic phenomena and phase transitions, and enables the development of electrically coupled spintronic devices, such as voltage-controlled magnetic memories with low operation energy. Previous studies on dilute magnetic semiconductors such as (Ga,Mn)As and (In,Mn)Sb have demonstrated large modulations of the Curie temperatures and coercive fields by altering the magnetic anisotropy and exchange interaction. Owing to their unique magnetic properties, the recently reported two-dimensional magnets provide a new system for studying these features. For instance, a bilayer of chromium triiodide (CrI3) behaves as a layered antiferromagnet with a magnetic field-driven metamagnetic transition. Here, we demonstrate electrostatic gate control of magnetism in CrI3 bilayers, probed by magneto-optical Kerr effect (MOKE) microscopy. At fixed magnetic fields near the metamagnetic transition, we realize voltage-controlled switching between antiferromagnetic and ferromagnetic states. At zero magnetic field, we demonstrate a time-reversal pair of layered antiferromagnetic states that exhibit spin-layer locking, leading to a linear dependence of their MOKE signals on gate voltage with opposite slopes. Here, our results allow for the exploration of new magnetoelectric phenomena and van der Waals spintronics based on 2D materials.},
doi = {10.1038/s41565-018-0121-3},
journal = {Nature Nanotechnology},
number = 30,
volume = 3,
place = {United States},
year = {2018},
month = {4}
}

Here, we examine the crystallographic and magnetic properties of single crystals of CrI 3, an easily cleavable, layered and insulating ferromagnet with a Curie temperature of 61 K. Our X-ray diffraction studies reveal a first-order crystallographic phase transition occurring near 210–220 K upon warming, with significant thermal hysteresis. The low-temperature structure is rhombohedral (Rmore » $$\bar{3}$$, BiI 3-type) and the high-temperature structure is monoclinic (C2/m, AlCl 3-type). Evidence for coupling between the crystallographic and magnetic degrees of freedom in CrI 3 was found; we observed an anomaly in the interlayer spacing at the Curie temperature and an anomaly in the magnetic susceptibility at the structural transition. First-principles calculations reveal the importance of proper treatment of the long-ranged interlayer forces, and van der Waals density functional theory does an excellent job of predicting the crystal structures and their relative stability. Our calculations suggest that the ferromagnetic order found in the bulk material may persist into monolayer form, suggesting that CrI 3 and other chromium trihalides may be promising materials for spintronic and magnetoelectronic research.« less

Understanding the magnetism at the interface between a ferromagnet and an insulator is essential because the commonly posited magnetic “dead” layer close to an interface can be problematic in magnetic tunnel junctions. Previously, degradation of the magnetic interface was attributed to charge discontinuity across the interface. In this paper, the interfacial magnetism was investigated using three identically prepared La 0.67Sr 0.33MnO 3 (LSMO) thin films grown on different oriented SrTiO 3 (STO) substrates by polarized neutron reflectometry. In all cases the magnetization at the LSMO/STO interface is larger than the film bulk. We show that the interfacial magnetization is largestmore » across the LSMO/STO interfaces with (001) and (111) orientations, which have the largest net charge discontinuities across the interfaces. In contrast, the magnetization of LSMO/STO across the (110) interface, the orientation with no net charge discontinuity, is the smallest of the three orientations. We show that a magnetically degraded interface is not intrinsic to LSMO/STO heterostructures. Finally, the approach to use different crystallographic orientations provides a means to investigate the influence of charge discontinuity on the interfacial magnetization.« less

We demonstrate reversible control of magnetization and anisotropy in La 0.67Sr 0.33MnO 3 films through interfacial oxygen migration. Gd metal capping layers deposited onto La 0.67Sr 0.33MnO 3 leach oxygen from the film through a solid-state redox reaction to form porous Gd 2O 3. X-ray absorption and polarized neutron reflectometry measurements show Mn valence alterations consistent with high oxygen vacancy concentrations, resulting in suppressed magnetization and increased coercive fields. Effects of the oxygen migration are observed both at the interface and also throughout the majority of a 40 nm thick film, suggesting extensive diffusion of oxygen vacancies. After Gd-capped Lamore »0.67Sr 0.33MnO 3 is exposed to atmospheric oxygen for a prolonged period of time, oxygen diffuses through the Gd 2O 3 layer and the magnetization of the La 0.67Sr 0.33MnO 3 returns to the uncapped value. In conclusion, these findings showcase perovskite heterostructures as ideal candidates for developing functional interfaces through chemically-induced oxygen migration.« less

Monolayer valley semiconductors, such as tungsten diselenide (WSe 2), possess valley pseudospin degrees of freedom that are optically addressable but degenerate in energy. Lifting the energy degeneracy by breaking time-reversal symmetry is vital for valley manipulation. This has been realized by directly applying magnetic fields or via pseudomagnetic fields generated by intense circularly polarized optical pulses. However, sweeping large magnetic fields is impractical for devices, and the pseudomagnetic fields are only effective in the presence of ultrafast laser pulses. The recent rise of two-dimensional (2D) magnets unlocks new approaches to controlling valley physics via van der Waals heterostructure engineering. Here,more » we demonstrate the wide continuous tuning of the valley polarization and valley Zeeman splitting with small changes in the laser-excitation power in heterostructures formed by monolayer WSe 2 and 2D magnetic chromium triiodide (CrI 3). The valley manipulation is realized via the optical control of the CrI 3 magnetization, which tunes the magnetic exchange field over a range of 20 T. Lastly, our results reveal a convenient new path toward the optical control of valley pseudospins and van der Waals magnetic heterostructures.« less

Interfacial magnetoelectric coupling (MEC) is a viable path to achieve electrical writing of magnetic information in spintronic devices. For the prototypical Fe/BaTiO 3 (BTO) system, only tiny changes of the interfacial Fe magnetic moment upon reversal of the BTO dielectric polarization have been predicted so far. Here, by using X-ray magnetic circular dichroism in combination with high resolution electron microscopy and first principles calculations, we report on an undisclosed physical mechanism for interfacial MEC in the Fe/BTO system. At the Fe/BTO interface, an ultrathin FeO x layer exists, whose magnetization can be electrically and reversibly switched on-off at room-temperature bymore » reversing the BTO polarization. The suppression / recovery of interfacial ferromagnetism results from the asymmetric effect that ionic displacements in BTO produces on the exchange coupling constants in the adjacent FeOx layer. The observed giant magnetoelectric response holds potential for optimizing interfacial MEC in view of efficient, low-power spintronic devices.« less